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Catalytic chemical vapor deposition synthesis of carbon nanotubes from methane on SiO supported Fe and Fe−Ni catalysts

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Title Catalytic chemical vapor deposition synthesis of carbon nanotubes from methane on SiO supported Fe and Fe−Ni catalysts
Names Nakagawa, Ayako (creator)
Kimura, Shoichi (advisor)
Date Issued 2008-08-05T18:11:11Z (iso8601)
Note Graduation date: 2009
Abstract Influences of operating conditions on the production of carbon nanotubes
(CNTs) were studied using Fe and Fe-Ni bimetallic catalysts supported on silicon
monoxide (SiO). The catalysts were prepared in three steps: (1) impregnation of SiO
powders with ferric nitride or combinations of ferric and nickel nitrides, (2) oxidation
of nitrides in an air stream, and (3) grinding the powders obtained. CNTs were
successfully synthesized by catalytic CVD using NH₃/CH₄ mixtures in a horizontal
tubular flow reactor. The following process parameters were varied to investigate their
effects on the growth rates of CNTs. The morphologies of catalysts and product CNTs
were observed by scanning electron microscope (SEM).
• The particle size of SiO,
• metal composition,
• metal loading,
• temperature for catalyst oxidation,
• extent of grinding of catalysts,
• NH₃ pretreatment time,
• reaction temperature for CNT growth,
• reaction time, and
• NH₃/CH₄ feed ratio.
Two different average sizes of SiO particles, 8 μm and 44 μm, were compared
based on the growth of CNTs in 5 min. Catalysts supported on 44 μm average sized
SiO particles demonstrated higher yields when they were not pretreated in an NH₃
stream. When 1 wt% Fe was loaded, aligned CNTs were formed, and a highest growth
rate per unit mass of catalyst was observed. The range of oxidation temperature to
achieve highest catalyst activities depended on metals and metal contents: 600 - 750°C
for 1 wt% Fe, 450 - 600°C for 3 wt% Fe, and 750 - 900°C for Fe-Ni. Grinding
catalysts for at least 3 minutes increased the growth rate of CNTs by approximately 40
percent. The growth of CNTs was enhanced when no NH₃ pretreatment of catalysts
was carried out, regardless of metals and metal contents. However, CNTs did not grow
appreciably from methane without ammonia. An NH₃/CH₄ feed ratio of 0.15 - 0.25
was observed to yield highest growth rates. The reaction temperature to achieve
highest CNT growth rates was found to be in the range between 990 and 1000 °C. The
growth of CNTs was not linear but decreased with reaction time.
Genre Thesis
Topic carbon nanotubes
Identifier http://hdl.handle.net/1957/9151

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